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Physical Origin of the Mechanochemical Coupling at Interfaces
Zhuohan Li1, Izabela Szlufarska1
1Department of Materials Science and Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706-1595, USA.
The mechanochemical response of material interfaces is influenced by both interface deformation and the underlying solid. Bulk elastic deformation significantly contributes to the activation volume, challenging previous assumptions.
Area of Science:
- Materials Science
- Computational Chemistry
- Surface Science
Background:
- Mechanochemistry studies the chemical reactions induced by mechanical force.
- Understanding material interface behavior under stress is crucial for various applications.
- Previous studies often focused solely on interfacial bond contributions to mechanochemical responses.
Purpose of the Study:
- To investigate the physical origins of the mechanochemical response at material interfaces.
- To quantify the contributions of interface deformation and bulk solid deformation.
- To re-evaluate the commonly assumed dominance of interfacial contributions.
Main Methods:
- Density functional theory (DFT) calculations were employed.
- Analysis of stress distribution and elastic deformation within bulk materials.
- Decomposition of mechanochemical response into interfacial and bulk contributions.
Main Results:
- Mechanochemical response is a sum of interfacial bond deformation and bulk solid contribution.
- Bulk elastic deformation significantly impacts activation volume, potentially dominating interfacial effects.
- Contact geometry and material stiffness dictate the relative contributions.
Conclusions:
- The elastic deformation of the surrounding bulk plays a significant role in the activation volume.
- Finite activation volumes and mechanochemical responses are expected due to bulk effects.
- Variability in experimental activation volumes may stem from differing bulk vs. interface contributions.
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